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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 9 ( 2022-05-05), p. 5877-5924
    Abstract: Abstract. Megacities and other major population centres (MPCs) worldwide are major sources of air pollution, both locally as well as downwind. The overall assessment and prediction of the impact of MPC pollution on tropospheric chemistry are challenging. The present work provides an overview of the highlights of a major new contribution to the understanding of this issue based on the data and analysis of the EMeRGe (Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales) international project. EMeRGe focuses on atmospheric chemistry, dynamics, and transport of local and regional pollution originating in MPCs. Airborne measurements, taking advantage of the long range capabilities of the High Altitude and LOng Range Research Aircraft (HALO, https://www.halo-spp.de, last access: 22 March 2022), are a central part of the project. The synergistic use and consistent interpretation of observational data sets of different spatial and temporal resolution (e.g. from ground-based networks, airborne campaigns, and satellite measurements) supported by modelling within EMeRGe provide unique insight to test the current understanding of MPC pollution outflows. In order to obtain an adequate set of measurements at different spatial scales, two field experiments were positioned in time and space to contrast situations when the photochemical transformation of plumes emerging from MPCs is large. These experiments were conducted in summer 2017 over Europe and in the inter-monsoon period over Asia in spring 2018. The intensive observational periods (IOPs) involved HALO airborne measurements of ozone and its precursors, volatile organic compounds, aerosol particles, and related species as well as coordinated ground-based ancillary observations at different sites. Perfluorocarbon (PFC) tracer releases and model forecasts supported the flight planning, the identification of pollution plumes, and the analysis of chemical transformations during transport. This paper describes the experimental deployment and scientific questions of the IOP in Europe. The MPC targets – London (United Kingdom; UK), the Benelux/Ruhr area (Belgium, the Netherlands, Luxembourg and Germany), Paris (France), Rome and the Po Valley (Italy), and Madrid and Barcelona (Spain) – were investigated during seven HALO research flights with an aircraft base in Germany for a total of 53 flight hours. An in-flight comparison of HALO with the collaborating UK-airborne platform Facility for Airborne Atmospheric Measurements (FAAM) took place to assure accuracy and comparability of the instrumentation on board. Overall, EMeRGe unites measurements of near- and far-field emissions and hence deals with complex air masses of local and distant sources. Regional transport of several European MPC outflows was successfully identified and measured. Chemical processing of the MPC emissions was inferred from airborne observations of primary and secondary pollutants and the ratios between species having different chemical lifetimes. Photochemical processing of aerosol and secondary formation or organic acids was evident during the transport of MPC plumes. Urban plumes mix efficiently with natural sources as mineral dust and with biomass burning emissions from vegetation and forest fires. This confirms the importance of wildland fire emissions in Europe and indicates an important but discontinuous contribution to the European emission budget that might be of relevance in the design of efficient mitigation strategies. The present work provides an overview of the most salient results in the European context, with these being addressed in more detail within additional dedicated EMeRGe studies. The deployment and results obtained in Asia will be the subject of separate publications.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 2
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 123, No. 18 ( 2018-09-27)
    Abstract: Problems of MAX‐DOAS retrievals of tropospheric O 3 are clarified and mostly solved New MAX‐DOAS retrieval methods of vertical profiles of tropospheric O 3 are developed The feasibility of the new methods is proven and deficiencies are described for future research
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2018
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    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 3 ( 2023-02-03), p. 1893-1918
    Abstract: Abstract. The number of large urban agglomerations is steadily increasing worldwide. At a local scale, their emissions lead to air pollution, directly affecting people's health. On a global scale, their emissions lead to an increase of greenhouse gases, affecting climate. In this context, in 2017 and 2018, the airborne campaign EMeRGe (Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales) investigated emissions of European and Asian major population centres (MPCs) to improve the understanding and predictability of pollution outflows. Here, we present two methods to identify and characterise pollution outflows probed during EMeRGe. First, we use a set of volatile organic compounds (VOCs) as chemical tracers to characterise air masses by specific source signals, i.e. benzene from anthropogenic pollution of targeted regions, acetonitrile from biomass burning (BB, primarily during EMeRGe-Asia), and isoprene from fresh biogenic signals (primarily during EMeRGe-Europe. Second, we attribute probed air masses to source regions and estimate their individual contribution by constructing and applying a simple emission uptake scheme for the boundary layer which combines FLEXTRA back trajectories and EDGAR carbon monoxide (CO) emission rates (acronyms are provided in the Appendix). During EMeRGe-Europe, we identified anthropogenic pollution outflows from northern Italy, southern Great Britain, the Belgium–Netherlands–Ruhr (BNR) area and the Iberian Peninsula. Additionally, our uptake scheme indicates significant long-range transport of pollution from the USA and Canada. During EMeRGe-Asia, the pollution outflow is dominated by sources in China and Taiwan, but BB signals from Southeast Asia and India contribute as well. Outflows of pre-selected MPC targets are identified in less than 20 % of the sampling time, due to restrictions in flight planning and constraints of the measurement platform itself. Still, EMeRGe combines in a unique way near- and far-field measurements, which show signatures of local and distant sources, transport and conversion fingerprints, and complex air mass compositions. Our approach provides a valuable classification and characterisation of the EMeRGe dataset, e.g. for BB and anthropogenic influence of potential source regions and paves the way for a more comprehensive analysis and various model studies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
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  • 4
    Online Resource
    Online Resource
    Springer Science and Business Media LLC ; 2014
    In:  Scientific Reports Vol. 4, No. 1 ( 2014-07-30)
    In: Scientific Reports, Springer Science and Business Media LLC, Vol. 4, No. 1 ( 2014-07-30)
    Abstract: We report on the evolution of tropospheric nitrogen dioxide (NO 2 ) over Spain, focusing on the densely populated cities of Barcelona, Bilbao, Madrid, Sevilla and Valencia, during 17 years, from 1996 to 2012. This data series combines observations from in-situ air quality monitoring networks and the satellite-based instruments GOME and SCIAMACHY. The results in these five cities show a smooth decrease in the NO 2 concentrations of ~2% per year in the period 1996–2008, due to the implementation of emissions control environmental legislation and a more abrupt descend of ~7% per year from 2008 to 2012 as a consequence of the economic recession. In the whole Spanish territory the NO 2 levels have decreased by ~22% from 1996 to 2012. Statistical analysis of several economic indicators is used to investigate the different factors driving the NO 2 concentration trends over Spain during the last two decades.
    Type of Medium: Online Resource
    ISSN: 2045-2322
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2014
    detail.hit.zdb_id: 2615211-3
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  • 5
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 3 ( 2017-03-07), p. 759-782
    Abstract: Abstract. Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (〈  0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2505596-3
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 10, No. 10 ( 2017-10-12), p. 3719-3742
    Abstract: Abstract. In order to promote the development of the passive DOAS technique the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) was held at the Max Planck Institute for Chemistry in Mainz, Germany, from June to October 2013. Here, we systematically compare the differential slant column densities (dSCDs) of nitrous acid (HONO) derived from measurements of seven different instruments. We also compare the tropospheric difference of SCDs (delta SCD) of HONO, namely the difference of the SCDs for the non-zenith observations and the zenith observation of the same elevation sequence. Different research groups analysed the spectra from their own instruments using their individual fit software. All the fit errors of HONO dSCDs from the instruments with cooled large-size detectors are mostly in the range of 0.1 to 0.3  ×  1015 molecules cm−2 for an integration time of 1 min. The fit error for the mini MAX-DOAS is around 0.7  ×  1015 molecules cm−2. Although the HONO delta SCDs are normally smaller than 6  ×  1015 molecules cm−2, consistent time series of HONO delta SCDs are retrieved from the measurements of different instruments. Both fits with a sequential Fraunhofer reference spectrum (FRS) and a daily noon FRS lead to similar consistency. Apart from the mini-MAX-DOAS, the systematic absolute differences of HONO delta SCDs between the instruments are smaller than 0.63  ×  1015 molecules cm−2. The correlation coefficients are higher than 0.7 and the slopes of linear regressions deviate from unity by less than 16 % for the elevation angle of 1°. The correlations decrease with an increase in elevation angle. All the participants also analysed synthetic spectra using the same baseline DOAS settings to evaluate the systematic errors of HONO results from their respective fit programs. In general the errors are smaller than 0.3  ×  1015 molecules cm−2, which is about half of the systematic difference between the real measurements.The differences of HONO delta SCDs retrieved in the selected three spectral ranges 335–361, 335–373 and 335–390 nm are considerable (up to 0.57  ×  1015 molecules cm−2) for both real measurements and synthetic spectra. We performed sensitivity studies to quantify the dominant systematic error sources and to find a recommended DOAS setting in the three spectral ranges. The results show that water vapour absorption, temperature and wavelength dependence of O4 absorption, temperature dependence of Ring spectrum, and polynomial and intensity offset correction all together dominate the systematic errors. We recommend a fit range of 335–373 nm for HONO retrievals. In such fit range the overall systematic uncertainty is about 0.87  ×  1015 molecules cm−2, much smaller than those in the other two ranges. The typical random uncertainty is estimated to be about 0.16  ×  1015 molecules cm−2, which is only 25 % of the total systematic uncertainty for most of the instruments in the MAD-CAT campaign. In summary for most of the MAX-DOAS instruments for elevation angle below 5°, half daytime measurements (usually in the morning) of HONO delta SCD can be over the detection limit of 0.2  ×  1015 molecules cm−2 with an uncertainty of  ∼  0.9  ×  1015 molecules cm−2.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2505596-3
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 15 ( 2019-08-13), p. 10257-10278
    Abstract: Abstract. Trace gas maps retrieved from satellite measurements show enhanced levels of the atmospheric volatile organic compounds formaldehyde (HCHO) and glyoxal (CHOCHO) over the Atlantic Ocean. To validate the spatial distribution of this continental outflow, ship-based measurements were taken during the Continental Outflow of Pollutants towards the MArine tRoposphere (COPMAR) project. A Multi-AXis Differential Optical Absorption Spectrometer (MAX-DOAS) was operated aboard the research vessel (RV) Maria S. Merian during cruise MSM58/2. This cruise was conducted in October 2016 from Ponta Delgada (Azores) to Cape Town (South Africa), crossing between Cabo Verde and the African continent. The instrument was continuously scanning the horizon, looking towards the African continent. Enhanced levels of HCHO and CHOCHO were found in the area of expected outflow during this cruise. The observed spatial gradients of HCHO and CHOCHO along the cruise track agree with the spatial distributions from satellite measurements and the Model for OZone and Related chemical Tracers version 4 (MOZART-4) model simulations. The continental outflow from the African continent is observed in an elevated layer, higher than 1000 m, and probably originates from biogenic emissions or biomass burning according to FLEXible PARTicle dispersion model (FLEXPART) emission sensitivities.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Measurement Techniques Vol. 11, No. 5 ( 2018-05-14), p. 2769-2795
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 11, No. 5 ( 2018-05-14), p. 2769-2795
    Abstract: Abstract. In this study, we present a novel nitrogen dioxide (NO2) differential optical absorption spectroscopy (DOAS) retrieval in the ultraviolet (UV) spectral range for observations from the Global Ozone Monitoring Instrument 2 on board EUMETSAT's MetOp-A (GOME-2A) satellite. We compare the results to those from an established NO2 retrieval in the visible (vis) spectral range from the same instrument and investigate how differences between the two are linked to the NO2 vertical profile shape in the troposphere.As expected, radiative transfer calculations for satellite geometries show that the sensitivity close to the ground is higher in the vis than in the UV spectral range. Consequently, NO2 slant column densities (SCDs) in the vis are usually higher than in the UV if the NO2 is close to the surface. Therefore, these differences in NO2 SCDs between the two spectral ranges contain information on the vertical distribution of NO2 in the troposphere. We combine these results with radiative transfer calculations and simulated NO2 fields from the TM5-MP chemistry transport model to evaluate the simulated NO2 vertical distribution.We investigate regions representative of both anthropogenic and biomass burning NO2 pollution. Anthropogenic air pollution is mostly located in the boundary layer close to the surface, which is reflected by large differences between UV and vis SCDs of  ∼  60 %. Biomass burning NO2 in contrast is often uplifted into elevated layers above the boundary layer. This is best seen in tropical Africa south of the Equator, where the biomass burning NO2 is well observed in the UV, and the SCD difference between the two spectral ranges is only  ∼  36 %. In tropical Africa north of the Equator, however, the biomass burning NO2 is located closer to the ground, reducing its visibility in the UV.While not enabling a full retrieval of the vertical NO2 profile shape in the troposphere, our results can help to constrain the vertical profile of NO2 in the lower troposphere and, when analysed together with simulated NO2 fields, can help to better interpret the model output.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2505596-3
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  • 9
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 11, No. 4 ( 2018-04-26), p. 2395-2426
    Abstract: Abstract. On board the Copernicus Sentinel-5 Precursor (S5P) platform, the TROPOspheric Monitoring Instrument (TROPOMI) is a double-channel, nadir-viewing grating spectrometer measuring solar back-scattered earthshine radiances in the ultraviolet, visible, near-infrared, and shortwave infrared with global daily coverage. In the ultraviolet range, its spectral resolution and radiometric performance are equivalent to those of its predecessor OMI, but its horizontal resolution at true nadir is improved by an order of magnitude. This paper introduces the formaldehyde (HCHO) tropospheric vertical column retrieval algorithm implemented in the S5P operational processor and comprehensively describes its various retrieval steps. Furthermore, algorithmic improvements developed in the framework of the EU FP7-project QA4ECV are described for future updates of the processor. Detailed error estimates are discussed in the light of Copernicus user requirements and needs for validation are highlighted. Finally, verification results based on the application of the algorithm to OMI measurements are presented, demonstrating the performances expected for TROPOMI.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 10
    In: Advances in Space Research, Elsevier BV, Vol. 48, No. 9 ( 2011-11), p. 1551-1564
    Type of Medium: Online Resource
    ISSN: 0273-1177
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2011
    detail.hit.zdb_id: 2023311-5
    SSG: 16,12
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