Global, regional and seasonal analysis of total ozone trends derived from the 1995–2020 GTO-ECV climate data record

We present an updated perspective on near-global total ozone trends for the period 1995–2020. We use the GOME-type (Global Ozone Monitoring Experiment) Total Ozone Essential Climate Variable (GTO-ECV) satellite data record which has been extended and generated as part of the European Space Agency's Climate Change Initiative (ESA-CCI) and European Union Copernicus Climate Change Service (EU-C3S) ozone projects. The focus of our work is to examine the regional patterns and seasonal dependency of the ozone trend. In the Southern Hemisphere we found regions that indicate statistically significant positive trends increasing from 0.6 ± 0.5(2σ) % per decade in the subtropics to 1.0 ± 0.9 % per decade in the middle latitudes and 2.8 ± 2.6 % per decade in the latitude band 60–70∘ S. In the middle latitudes of the Northern Hemisphere the trend exhibits distinct regional patterns, i.e., latitudinal and longitudinal structures. Significant positive trends (∼ 1.5 ± 1.0 % per decade) over the North Atlantic region, as well as barely significant negative trends (−1.0 ± 1.0 % per decade) over eastern Europe, were found. Moreover, these trends correlate with long-term changes in tropopause pressure. Total ozone trends in the tropics are not statistically significant. Regarding the seasonal dependence of the trends we found only very small variations over the course of the year. However, we identified different behavior depending on latitude. In the latitude band 40–70∘ N the positive trend maximizes in boreal winter from December to February. In the middle latitudes of the Southern Hemisphere (35–50∘ S) the trend is maximum from March to May. Further south toward the high latitudes (55–70∘ S) the trend exhibits a relatively strong seasonal cycle which varies from 2 % per decade in December and January to 3.8 % per decade in June and July

Trends of tropical tropospheric ozone from 20 years of European satellite measurements and perspectives for the Sentinel-5 Precursor

In preparation of the TROPOMI/S5P launch in early 2017, a tropospheric ozone retrieval based on the convective cloud differential method was developed. For intensive tests we applied the algorithm to the total ozone columns and cloud data of the satellite instruments GOME, SCIAMACHY, OMI, GOME-2A and GOME-2B. Thereby a time series of 20 years (1995–2015) of tropospheric column ozone was generated. To have a consistent total ozone data set for all sensors, one common retrieval algorithm, namely GODFITv3, was applied and the L1 reflectances were also soft calibrated. The total ozone columns and the cloud data were input into the tropospheric ozone retrieval. However, the tropical tropospheric column ozone (TCO) for the individual instruments still showed small differences and, therefore, we harmonised the data set. For this purpose, a multilinear function was fitted to the averaged difference between SCIAMACHY's TCO and those from the other sensors. The original TCO was corrected by the fitted offset. GOME-2B data were corrected relative to the harmonised data from OMI and GOME-2A. The harmonisation leads to a better agreement between the different instruments. Also, a direct comparison of the TCO in the overlapping periods proves that GOME-2A agrees much better with SCIAMACHY after the harmonisation. The improvements for OMI were small. Based on the harmonised observations, we created a merged data product, containing the TCO from July 1995 to December 2015. A first application of this 20-year record is a trend analysis. The tropical trend is 0.7 ± 0.12 DU decade−1. Regionally the trends reach up to 1.8 DU decade−1 like on the African Atlantic coast, while over the western Pacific the tropospheric ozone declined over the last 20 years with up to 0.8 DU decade−1. The tropical tropospheric data record will be extended in the future with the TROPOMI/S5P data, where the TCO is part of the operational products

Constraining industrial ammonia emissions using hyperspectral infrared imaging

Atmospheric emissions of reactive nitrogen in the form of nitrogen dioxide (NO) and ammonia (NH) worsen air quality and upon deposition, dramatically affect the environment. Recent infrared satellite measurements have revealed that NH emitted by industries are an important and underestimated emission source. Yet, to assess these emissions, current satellite sounders are severely limited by their spatial resolution. In this paper, we analyse measurement data recorded in a series of imaging surveys that were conducted over industries in the Greater Berlin area (Germany). On board the aircraft were the Telops Hyper-Cam LW, targeting NH measurements in the longwave infrared at a resolution of 4 m and the SWING+ spectrometer targeting NO measurements in the UV–Vis at a resolution of 180 m. Two flights were carried out over German’s largest production facility of synthetic NH , urea and other fertilizers. In both cases, a large NH plume was observed originating from the factory. Using a Gaussian plume model to take into account plume rise and dispersion, coupled with well-established radiative transfer and inverse methods, we retrieve vertical column densities. From these, we calculate NH emission fluxes using the integrated mass enhancement and cross-sectional flux methods, yielding consistent emissions of the order of 2200 t yr−1 for both flights, assuming constant fluxes across the year. These estimates are about five times larger than those reported in the European Pollutant Release and Transfer Register (E-PRTR) for this plant. In the second campaign, a co-emitted NO plume was measured, likely related to the production of nitric acid at the plant. A third flight was carried out over an area comprising the cities of Staßfurt and Bernburg. Several small NH plumes were seen, one over a production facility of mineral wool insulation, one over a sugar factory and two over the soda ash plants in Staßfurt and Bernburg. A fifth and much larger plume was seen to originate from the sedimentation basins associated with the soda ash plant in Staßfurt, indicating rapid volatilization of ammonium rich effluents. We use the different measurement campaigns to simulate measurements of Nitrosat, a potential future satellite sounder dedicated to the sounding of reactive nitrogen at a resolution of 500 m. We demonstrate that such measurements would allow accurately constraining emissions in a single overpass, overcoming a number of important drawbacks of current satellite sounders

Regulated large-scale annual shutdown of Amazonian isoprene emissions?

We perform Empirical Orthogonal Function (EOF) analysis on 12 years of global GOME and SCIAMACHY formaldehyde (HCHO) column observations to determine the most significant spatial and temporal HCHO variations. In most regions, we find that HCHO variability is predominantly driven by seasonal variations of biogenie emissions and biomass burning. However, unusually low HCHO columns are consistently observed over the Amazon rainforest during the transition from the wet-to-dry seasons. We use MODIS leaf area and enhanced vegetation indices, to show variations in vegetation are consistent with the observed decrease in HCHO during this period (correlations of 0.69 and 0.67, respectively). Based on this evidence, we suggest isoprene emitting vegetation experience widespread leaf flushing (new leaf growth) prior to the dry season, resulting in a large-scale annual shutdown of Amazonian isoprene emissions. © 2009

Record low ozone values over the Arctic in boreal spring 2020

. Ozone data derived from the Tropospheric Monitoring Instrument (TROPOMI) sensor on board the Sentinel- 5 Precursor satellite show exceptionally low total ozone columns in the polar region of the Northern Hemisphere (Arctic) in spring 2020. Minimum total ozone column values around or below 220 Dobson units (DU) were seen over the Arctic for 5 weeks in March and early April 2020. Usually the persistence of such low total ozone column values in spring is only observed in the polar Southern Hemisphere (Antarctic) and not over the Arctic

Two decades of homogenized satellite ozone measurements for climate services

Since the launch of GOME onboard ERS-2 in 1995 total and tropospheric ozone have been derived from European satellite instruments. In the framework of the ESA CCI and the EU ECMWF C3S projects, BIRA generates total ozone products from the satellite sensors GOME, SCIAMACHY, OMI, and GOME-2 using the GODFIT algorithm and DLR is responsible for harmonizing the total column data from all these sensors and generating a merged product, which encompasses more than two decades of global total ozone observations. Additionally, tropospheric ozone columns form the European sensors are generated by DLR using the convective cloud differential algorithm. Total and tropospheric ozone from GOME-2 onboard MetOp-A and -B are operational products from the EUMETSAT AC-SAF and within the ESA CCI project the tropical tropospheric ozone products from GOME, SCIAMACHY, OMI, and GOME-2 were harmonized and a merged data product was delivered and has been updated regularly. On a global scale a slight increase in total ozone columns is observed over the years since 1995 until today indicating that the total ozone starts to emerge into the expected recovery phase. Tropospheric data from the last 22 years show a slightly increasing trend with strong regional variations especially in the tropical eastern Pacific and Atlantic Ocean. These unique ozone datasets will be extended during the next two decades with measurements from the EU Copernicus missions Sentinel-5 Precursors (successfully launched in October 2017) and the future Sentinel-4 and Sentinel-5 missions

Advanced exploitation of Ground-Based measurements for Atmospheric Chemistry and Climate Applications "AGACC"

We live in an era in which human activities are causing significant changes to the atmospheric environment which result in local to global consequences on the ecosystems. Changes in the atmospheric composition impact our climate via chemical and dynamical feedback mechanisms; in many instances they also affect air quality, and the health of the biosphere. Monitoring and understanding those changes and their consequences is fundamental to establish adequate actions for adaptation to and mitigation of the environmental changes. Furthermore, after implementation of regulatory measures like the Montreal Protocol, it is necessary to verify whether the measures are effective. This can only be achieved if we have adequate detection methods and a reliable long record of a series of key geophysical parameters. Thus the AGACC project contributes to the provision of basic new knowledge regarding the atmospheric composition and its changes, based on advanced groundbased monitoring, in combination with satellite and numerical modelling data. Its results are integrated in ongoing international research programmes. The general objective of AGACC has been to improve and extend the groundbased detection capabilities for a number of climate-related target species and, based hereupon, analyse past and present observations to derive new information about the atmospheric composition, its variability and long-term changes. Despite the advent of a growing and more performant fleet of Earth Observation satellites, ground-based observations are still indispensable to (1) guarantee long-term continuity, homogeneity and high quality of the data, and (2) to underpin the satellite data for calibration and (long-term) validation. A first target gas is atmospheric water vapour. It is the key trace gas controlling weather and climate. It is also the most important greenhouse gas in the Earth’s atmosphere. Its amount and vertical distribution are changing, but how and why? Especially in the upper troposphere - lower stratosphere, the radiative effects of changes in the water vapour are significant and should be quantified. The measurement of water vapour is a hot topic since several years. It is a challenge, because water vapour exhibits a large gradient in its concentration when going from the ground to the stratosphere, and because it is highly variable in time and space. For example, we have found that the time scale of the variations of the total water vapour amount at Jungfraujoch is in the order of minutes. In AGACC, we have therefore investigated various experimental techniques to measure the concentration of water vapour in the atmosphere, focusing on the total column as well as on the vertical distribution in the troposphere up to the lower stratosphere. The retrieval of water vapour vertical profiles and total columns from ground-based FTIR data has been initiated at three very different stations where correlative data for verification are available, namely Ukkel (± sea level, mid-latitude), Ile de La Réunion (± sea level, tropical) and Jungfraujoch (high altitude, mid-latitude), with promising results. In particular, at Jungfraujoch, it has been demonstrated that the precision of the FTIR integrated water vapour (IWV) measurements is of order 2%. The capability to retrieve individual isotopologues of water vapour, and to monitor their daily and diurnal variations, has also been demonstrated. This could open new ways to study in the future the role of water vapour in the radiative balance, the global circulation, precipitation etc. We also started joint exploitation of ground-based FTIR and satellite IASI data for water vapour and its isotopologues, in order to exploit fully the potential of the existing instrumentation. A correction method for the radiosoundings at Ukkel has been successfully implemented, resulting in a homogeneous and reliable time series from 1990 to 2008 from which trends in upper troposphere humidity (UTH) and tropopause characteristics have been derived. One observes a rising UTH until September 2001, followed by a decline, accompanied by a descent and heating of the tropopause up to the turning point and an ascent and cooling afterwards. The changes after September 2001 in the upper troposphere can be explained by surface heating and convective uplift. At Jungfraujoch, one does not observe any significant trend in the total water vapour abundance above the station over the 1988-2010 time period, although significant positive summer and negative winter trends have been detected. We have made a quantitative statistical comparison between ground-based FTIR, CIMEL, GPS and integrated (corrected) radio sounding measurements of the IWV at Ukkel. This work is important to better characterize the different sensors in order to exploit together different observations made by different instruments. A second target species is atmospheric aerosol. There is a very large variety of aerosol both from natural or anthropogenic origin. One of the reasons why they are so important is that they affect the optical properties of the atmosphere. In particular, it has been demonstrated in previous studies that the aerosols have a large impact on the quantity of harmful UV-B radiation received at the Earth’s surface. The latest IPCC Report also stressed that the radiative forcing caused by atmospheric aerosols is one of the largest uncertainties in determining the total radiative forcing in the atmosphere. Better monitoring capabilities of aerosol properties can therefore improve our understanding and forecasting of the atmospheric processes and evolution, and in particular of UV-B and climate changes. Several measurement techniques are now operational in the AGACC consortium for the ground-based monitoring of aerosol properties. These are the Brewer spectrometer and CIMEL observations at Ukkel, the latter contributing also to the AERONET network since July 2006, and the newly developed MAXDOAS observations. Unlike CIMEL and Brewer measurements, that provide the total Aerosol Optical Depth, it has been demonstrated that the MAXDOAS measurements also provide additional information about the vertical distribution of the aerosol extinction in the lowest kilometres of the troposphere. A better understanding of the ultimate capabilities of MAXDOAS aerosol remote sensing has been gained through participation to the international CINDI campaign (Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments ) in summer 2009. The combination of Brewer, CIMEL and MAXDOAS instruments gives us a remote-sensing dataset that will enable a more comprehensive characterization of the tropospheric aerosol optical properties. The usefulness of these aerosol observations has already been demonstrated in the improvement of the UVindex predictions for the general public. Another application is their use as input data in the retrieval of vertical profiles of tropospheric pollutants from MAXDOAS measurements, like tropospheric NO2 and formaldehyde. Third we have focused on a few climate-related trace gases. Changing greenhouse gas and aerosol concentrations directly affect the radiative budget of the atmosphere, and therefore climate. But many species known as pollutants like carbon monoxide (CO), nitrogen oxides (NOx) and hydrocarbons, - often related to fossil fuel or biomass burning -, also affect climate through their role in chemical reactions that produce tropospheric ozone, which is a well-known greenhouse gas, or that modify the lifetime of gases like methane, or the oxidation capacity of the atmosphere. Therefore in AGACC, we have focused on the measurement of a number of trace gases that are subject to changing concentrations, that directly or indirectly affect climate, and that are either difficult to monitor or that have not yet been measured from the ground. We have included attempts to observe distinctly some isotopologues, because the isotopic ratios observed in an airmass provide information on its history, and because the FTIR solar absorption measurements provide a rather unique capability hereto. The investigated species are the isotopologues of CH4 and CO, and hydrogen cyanide (HCN), as examples of biomass burning tracers, some hydrocarbons like formaldehyde (HCHO), ethylene (C2H4) and acetylene (C2H2), and HCFC-142b, a replacement product for CFCs and a greenhouse gas. In many cases, retrieval strategies had to be adapted when going from one site to another with different atmospheric conditions, especially when the local humidity and abundances are very different as is the case between Jungfraujoch (dry, high altitude, mid-latitude) and Ile de La Réunion (humid, low altitude, low latitude). Still we have been able to show the feasibility of retrieving particular trace gas information even under difficult conditions. Many of our results have been compared to correlative data, to validate the approach and to gain complementary information. It is also important to note that the retrieval strategies developed in AGACC have regularly been presented to the global Network for the Detection of Atmospheric Composition Change (NDACC) UV-Vis and Infrared communities and have often been adopted by others or even proposed for adoption as a standard in the community (e.g., for hydrogen cyanide (HCN)). In particular: We have been able to study the seasonal variations of HCN at the Jungfraujoch and at Ile de La Réunion, and to show the dominant impact of biomass burning. Formaldehyde was studied in much detail at Ukkel, Jungfraujoch and Ile de la Réunion. The challenge for detection at Jungfraujoch is the small abundance (about 10 times smaller than at Ukkel and Ile de La Réunion); a particular observation strategy was developed successfully, resulting in a time series that already shows the day-to-day and seasonal variations. At Ile de La Réunion, comparisons of FTIR, MAXDOAS, satellite and model data have (1) shown the good agreement between the various data sets, but also, (2), the variability of HCHO (diurnal, seasonal, day-to-day), and (3), thanks to the complementarities of the various data sets, they have enabled us to learn more about the long-range transport of Non-methane Volatile Organic Compounds (NMVOCS, precursors of HCHO) and deficiencies in the models. It was shown that fast, direct transport of NMVOCS from Madagascar has a significant impact on the HCHO abundance and its variability at Ile de La Réunion, and that this is underestimated in the model. Significant progress was made as to the detection of 13CH4 and CH3D from ground-based FTIR observations, both at Jungfraujoch and Ile de La Réunion. To our knowledge, it is the first time that a d13C data set is derived from ground-based FTIR observations. More work is needed to improve the CH3D retrieval at Ile de La Réunion, and to interpret the results, in combination with models. Also for the first time, 12CO and 13CO have been retrieved individually at Jungfraujoch. The d13C time series shows significant seasonal and interannual changes. As to the hydrocarbon ethylene, it is shown that it can be detected at Jungfraujoch only in spectra at low solar elevation, given its small atmospheric abundance. Regarding acetylene, the observed time series at Jungfraujoch and Ile de La Réunion show clear seasonal variations and enhancements due to the impact of biomass burning events, correlated with enhancements in CO, C2H6 and HCN. It is not clear yet whether we can reliably retrieve the concentration of HCFC- 142b, a replacement product that is increasing strongly in the troposphere. New line parameters for the interfering species HFC-134a are required to confirm/infirm the preliminary results. This highlights again the importance of the laboratory work for providing such parameters. Improved line parameters have been obtained for water vapour and its isotopologues, ethylene and formic acid. These AGACC results have been integrated in the international spectroscopic databases. We also showed that line intensities available around 2096 cm–1 for the 13C16O isotopologue of carbon monoxide in the HITRAN database seem to be accurate to 2%. We failed to improve line intensities for the 13.6 μm region of acetylene. The new data sets that have been derived in AGACC from FTIR and MAXDOAS observations have been archived in the NDACC data centre, where they are available for users (generally modelers and satellite teams). In addition, they are stored locally and are available to users upon request. AGACC results have been reported to the international scientific community, via the literature, via integration in geophysical or spectroscopic databases, and via participation to international research initiatives like the Atmospheric Water Vapour in the Climate System (WAVACS) Cost Action, the International Space Science Institute (ISSI) Working Group on Atmospheric Water Vapour, the International Union of Pure and Applied Chemistry (IUPAC) project, the International CINDI campaign, etc. The results have already found important scientific applications. A few examples are worth mentioning: the re-evaluation of methane emissions in the tropics from SCIAMACHY based on the new H2O spectroscopy, and the improved retrievals of HCOOH from the satellite experiments ACE-FTS and IASI, and from the ground. In the longer-term, the AGACC results will no doubt benefit the research in atmospheric sciences –in particular in the monitoring of its composition changes–, which is the fundamental basis of environmental assessment reports for supporting policy makers.Advanced exploitation of ground-based measurements for atmospheric chemistry and climate applications "AGACC

Tropospheric ozone column data records based on total columns from GOME, SCIAMACHY, GOME-2, OMI and TROPOMI using CCD algorithm or in combination with BASCOE/MLS

A long-term tropospheric ozone time series has been generated for the tropical band (20°S to 20°N) based on convective cloud differential algorithm (CCD). Tropical tropospheric ozone columns were retrieved from several European sensors starting with observations by GOME in 1995 and including data from SCIAMACHY, OMI, GOME-2A and GOME-2B. It has now been extended by DLR with data from GOME-2C and TROPOMI and now encompasses 25 years. The tropospheric ozone retrieval for all data sets is based on the total columns retrieved with the GODFIT algorithm and associated cloud products. There are however some differences between the different tropospheric columns from the different sensors which have to be corrected for. For the CCD time series, we used SCIAMACHY data as reference and fitted an offset and a trend correction to the data of the other sensors. We estimated the trend based on the long-term time series. For the tropics an overall trend of +0.7 DU/decade was found in the data set until 2019, varying locally between -0.5 and 1.8 DU/decade. The second data record combines total ozone columns from TROPOMI with BASCOE stratospheric ozone profiles. BASCOE stratospheric ozone data is constrained by assimilated Aura MLS observation and it is provided with 3-hour time resolutions in NRT. We used the BASCOE NRT data set to calculate the stratospheric ozone columns for every day from April 2018 to December 2020 and subtracted it from the respective NRT total columns observed by TROPOMI. The TROPOMI NRT total ozone product was updated recently including a new surface albedo retrieval algorithm. An internal reanalysis of the NRT data was used to create a consistent tropospheric ozone data set. A comparison to ozone sondes showed a good agreement for most part of the world. For the GEMS validation the TROPOMI total ozone NRT algorithm is applied to selected the GEMS data. Also, the tropospheric ozone column might be retrieved based on the TROPOMI-BASCOE algorithm described above. Both the CCD and the TROPOMI-BASCOE tropospheric ozone data will be presented. Furthermore, first results for total and troposheric ozone columns of GEMS data using the TROPOMI algorithms might be shown

Level 1-to-2 Data Processor Version 3.0: A Major Upgrade of the GOME/ERS-2 Total Ozone Retrieval Algorithm,

Abstract The Global Ozone Monitoring Experiment (GOME) was launched in April 1995, and the GOME Data Processor (GDP) retrieval algorithm has processed operational total ozone amounts since July 1995. GDP Level 1-to-2 is based on the two-step Differential Optical Absorption Spectroscopy (DOAS) approach, involving slant column fitting followed by Air Mass Factor (AMF) conversions to vertical column amounts. We present a major upgrade of this algorithm to Version 3.0. GDP 3.0 was implemented in July 2002, and the 9-year GOME data record from July 1995 to December 2004 has been processed using this algorithm. The key component in GDP 3.0 is an iterative approach to AMF calculation, in which AMFs and corresponding vertical column densities are adjusted to reflect the true ozone distribution as represented by the fitted DOAS effective slant column. A neural networkensemble is used to optimize the fast and accurate parameterization of AMFs. We describe results of a recent validation exercise for the operational version of the total ozone algorithm; in particular, seasonal and meridian errors are reduced by a factor of two. On a global basis, GDP 3.0 ozone total column results lie between -2% and +4% of ground-based values for moderate solar zenith angles lower than 70°. A larger variability of about +5% and -8% is observed for higher solar zenith angles up to 90°. Copyright OCIS codes 01