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In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97 degrees N, 4.93 degrees E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O-4) and ozone (O-3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques. Netherlands Space Office (NSO); ESA through the CINDI-2 (ESA) project [4000118533/16/I-Sbo]; ESA through the FRM4DOAS (ESA) project [4000118181/16/I-EF]; EU 7th Framework Programme QA4ECV projectEuropean Union (EU) [607405]; Austrian Science Fund (FWF)Austrian Science Fund (FWF) [I 2296-N29]; Canadian Space Agency (AVATARS project); Natural Sciences and Engineering Research Council (PAHA project); Canada Foundation for InnovationCanada Foundation for Innovation; UVAS ("Ultraviolet and Visible Atmospheric Sounder") projects SEOSAT/INGENIO [ESP2015-71299-R]; DFG project RAPSODI [PL 193/17-1]; Centre National de la Recherche Scientifique (CNRS)Centre National de la Recherche Scientifique (CNRS); Centre National d'Etudes Spatiales (CNES)Centre National D'etudes Spatiales; National funding project HELADO [CTM2013-41311-P]; National funding project AVATAR [CGL2014-55230-R]; Russian Science FoundationRussian Science Foundation (RSF) [16-17-10275]; Russian Foundation for Basic ResearchRussian Foundation for Basic Research (RFBR) [16-05-01062, 18-35-00682]; ACTRIS-2 (H2020 grant) [654109]; NASA's Atmospheric Composition ProgramNational Aeronautics & Space Administration (NASA) [NASA-16-NUP2016-0001]; US National Science FoundationNational Science Foundation (NSF) [AGS-1620530]; NASANational Aeronautics & Space Administration (NASA); University of Bremen; DFG Research Center/Cluster of Excellence "The Ocean in the Earth System-MARUM"German Research Foundation (DFG); University of Bremen Institutional Strategy of the DFG; Luftblick through the ESA Pandonia Project; NASA Pandora Project at the Goddard Space Flight Center under NASA Headquarters' Tropospheric Composition Program CINDI-2 received funding from the Netherlands Space Office (NSO). Funding for this study was provided by ESA through the CINDI-2 (ESA contract no. 4000118533/16/I-Sbo) and FRM4DOAS (ESA contract no. 4000118181/16/I-EF) projects and partly within the EU 7th Framework Programme QA4ECV project (grant agreement no. 607405). The BOKU MAX-DOAS instrument was funded and the participation of Stefan F. Schreier was supported by the Austrian Science Fund (FWF): I 2296-N29. The participation of the University of Toronto team was supported by the Canadian Space Agency (through the AVATARS project) and the Natural Sciences and Engineering Research Council (through the PAHA project). The instrument was primarily funded by the Canada Foundation for Innovation and is usually operated at the Polar Environment Atmospheric Research Laboratory (PEARL) by the Canadian Network for the Detection of Atmospheric Change (CANDAC). Funding for CISC was provided by the UVAS ("Ultraviolet and Visible Atmospheric Sounder") projects SEOSAT/INGENIO, ESP2015-71299-R, MINECO-FEDER and UE. The activities of the IUP-Heidelberg were supported by the DFG project RAPSODI (grant no. PL 193/17-1). SAOZ and Mini-SAOZ instruments are supported by the Centre National de la Recherche Scientifique (CNRS) and the Centre National d'Etudes Spatiales (CNES). INTA recognises support from the National funding projects HELADO (CTM2013-41311-P) and AVATAR (CGL2014-55230-R). AMOIAP recognises support from the Russian Science Foundation (grant no. 16-17-10275) and the Russian Foundation for Basic Research (grant nos. 16-05-01062 and 18-35-00682). Ka L. Chan received transnational access funding from ACTRIS-2 (H2020 grant agreement no. 654109). Rainer Volkamer recognises funding from NASA's Atmospheric Composition Program (NASA-16-NUP2016-0001) and the US National Science Foundation (award AGS-1620530). Henning Finkenzeller is the recipient of a NASA graduate fellowship. Mihalis Vrekoussis recognises support from the University of Bremen and the DFG Research Center/Cluster of Excellence "The Ocean in the Earth System-MARUM". Financial support through the University of Bremen Institutional Strategy in the framework of the DFG Excellence Initiative is gratefully appreciated for Anja Schonhardt. Pandora instrument deployment was supported by Luftblick through the ESA Pandonia Project and NASA Pandora Project at the Goddard Space Flight Center under NASA Headquarters' Tropospheric Composition Program. The article processing charges for this open-access publication were covered by BK Scientific.

40 pags., 22 figs., 13 tabs., In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17¿d during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, the Netherlands (51.97¿¿N, 4.93¿¿E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were (1) to characterise and better understand the differences between a large number of multi-axis differential optical absorption spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, (2) to define a robust methodology for performance assessment of all participating instruments, and (3) to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen collision complex (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region, and NO2 in an additional (smaller) wavelength range in the visible region. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in a unique set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the selected reference (which is obtained from the median of either all data sets or a subset), and the rms error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the consistency between all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques., CINDI-2 received funding from the Netherlands Space Office (NSO). Funding for this study was provided by ESA through the CINDI-2 (ESA contract no. 4000118533/16/ISbo) and FRM4DOAS (ESA contract no. 4000118181/16/I-EF) projects and partly within the EU 7th Framework Programme QA4ECV project (grant agreement no. 607405). The BOKU MAX-DOAS instrument was funded and the participation of Stefan F. Schreier was supported by the Austrian Science Fund (FWF): I 2296-N29. The participation of the University of Toronto team was supported by the Canadian Space Agency (through the AVATARS project) and the Natural Sciences and Engineering Research Council (through the PAHA project). The instrument was primarily funded by the Canada Foundation for Innovation and is usually operated at the Polar Environment Atmospheric Research Laboratory (PEARL) by the Canadian Network for the Detection of Atmospheric Change (CANDAC). Funding for CISC was provided by the UVAS (“Ultraviolet and Visible Atmospheric Sounder”) projects SEOSAT/INGENIO, ESP2015-71299- R, MINECO-FEDER and UE. The activities of the IUP-Heidelberg were supported by the DFG project RAPSODI (grant no. PL 193/17-1). SAOZ and Mini-SAOZ instruments are supported by the Centre National de la Recherche Scientifique (CNRS) and the Centre National d’Etudes Spatiales (CNES). INTA recognises support from the National funding projects HELADO (CTM2013-41311-P) and AVATAR (CGL2014-55230-R). AMOIAP recognises support from the Russian Science Foundation (grant no. 16-17-10275) and the Russian Foundation for Basic Research (grant nos. 16-05- 01062 and 18-35-00682). Ka L. Chan received transnational access funding from ACTRIS-2 (H2020 grant agreement no. 654109). Rainer Volkamer recognises funding from NASA’s Atmospheric Composition Program (NASA-16-NUP2016-0001) and the US National Science Foundation (award AGS-1620530). Henning Finkenzeller is the recipient of a NASA graduate fellowship. Mihalis Vrekoussis recognises support from the University of Bremen and the DFG Research Center/Cluster of Excellence “The Ocean in the Earth System-MARUM”. Financial support through the University of Bremen Institutional Strategy in the framework of the DFG Excellence Initiative is gratefully appreciated for Anja Schönhardt. Pandora instrument deployment was supported by Luftblick through the ESA Pandonia Project and NASA Pandora Project at the Goddard Space Flight Center under NASA Headquarters’ Tropospheric Composition Program. The article processing charges for this open-access publication were covered by BK Scientific.

The QA4ECV (Quality Assurance for Essential Climate Variables) version 1.1 stratospheric and tropospheric NO2 vertical column density (VCD) climate data records (CDRs) from the OMI (Ozone Monitoring Instrument) satellite sensor are validated using NDACC (Network for the Detection of Atmospheric Composition Change) zenithscattered light differential optical absorption spectroscopy (ZSL-DOAS) and multi-axis DOAS (MAX-DOAS) data as a reference. The QA4ECV OMI stratospheric VCDs have a small bias of 0:2 Pmolec:cm-2 (5 % 10 %) and a dispersion of 0.2 to 1 Pmolec:cm-2 with respect to the ZSLDOAS measurements. QA4ECV tropospheric VCD observations from OMI are restricted to near-cloud-free scenes, leading to a negative sampling bias (with respect to the unrestricted scene ensemble) of a few peta molecules per square centimetre (Pmolec:cm-2) up to -10 Pmolec:cm-2 (-40 %) in one extreme high-pollution case. The QA4ECV OMI tropospheric VCD has a negative bias with respect to the MAX-DOAS data (-1 to -4 Pmolec:cm-2), which is a feature also found for the OMI OMNO2 standard data product. The tropospheric VCD discrepancies between satellite measurements and ground-based data greatly exceed the combined measurement uncertainties. Depending on the site, part of the discrepancy can be attributed to a combination of comparison errors (notably horizontal smoothing difference error), measurement/retrieval errors related to clouds and aerosols, and the difference in vertical smoothing and a priori profile assumptions.

In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants for a period of 17 days during the Second Cabauw Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2) that took place at Cabauw, The Netherlands (51.97° N, 4.93° E). We report on the outcome of the formal semi-blind intercomparison exercise, which was held under the umbrella of the Network for the Detection of Atmospheric Composition Change (NDACC) and the European Space Agency (ESA). The three major goals of CINDI-2 were to characterise and better understand the differences between a large number of Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) and zenith-sky DOAS instruments and analysis methods, to discuss the performance of the various types of instruments and to contribute to a harmonisation of the measurement settings and retrieval methods. This, in turn, creates the capability to produce consistent high-quality ground-based data sets, which are an essential requirement to generate reliable long-term measurement time series suitable for trend analysis and satellite data validation. The data products investigated during the semi-blind intercomparison are slant columns of nitrogen dioxide (NO2), the oxygen dimer (O4) and ozone (O3) measured in the UV and visible wavelength region, formaldehyde (HCHO) in the UV spectral region and NO2 in an additional (smaller) wavelength range in the visible. The campaign design and implementation processes are discussed in detail including the measurement protocol, calibration procedures and slant column retrieval settings. Strong emphasis was put on the careful alignment and synchronisation of the measurement systems, resulting in an unprecedented set of measurements made under highly comparable air mass conditions. The CINDI-2 data sets were investigated using a regression analysis of the slant columns measured by each instrument and for each of the target data products. The slope and intercept of the regression analysis respectively quantify the mean systematic bias and offset of the individual data sets against the reference, and the RMS error provides an estimate of the measurement noise or dispersion. These three criteria are examined and for each of the parameters and each of the data products, performance thresholds are set and applied to all the measurements. The approach presented here has been developed based on heritage from previous intercomparison exercises. It introduces a quantitative assessment of the measurement performance of all the participating instruments for the MAX-DOAS and zenith-sky DOAS techniques.

Aerosols are particles in the solid or liquid phase that are suspended in the atmosphere. They have an important influence on the atmospheric chemistry and physics, affect the tropospheric chemical composition, can reduce visibility and have important impacts on human health. Aerosols also influence the Earth’s radiation budget. Although a lot of research has been done to investigate the influence of aerosols on the climate, they remain key contributors to the uncertainties in current climate studies due to the lack of information concerning their temporal and spatial distribution. One of the parameters that is of importance to understand the influence of aerosols is the aerosol optical depth (AOD), an integral measurement of the combined aerosol scattering and absorption in the atmospheric column. The first part of this PhD describes an adapted and improved method for the retrieval of AOD values using sun scan measurements from a Brewer spectrophotometer at 340 nm at Uccle. The retrieved AOD values are subjected to a cloud screening technique and are compared to quasi simultaneous, collocated CIMEL AOD values. The good agreement between both instruments highlights that the Brewer is largely sensitive to AOD at 340 nm and it justifies its use in sun scan mode to expand the AOD retrieval network of instruments. The monthly and seasonal behavior of the retrieved AOD values is also studied in this work and our results agree with results found in literature.Another point of concern in scientific communities is the known adverse effect of UV radiation on human health, the biosphere and atmospheric chemistry. Apart from its obvious relation with global solar radiation and ozone, the amount of UV radiation that reaches the surface of the Earth also depends on the characteristics and quantity of aerosols in the atmosphere and accuracy in UV prediction can be improved if the influence of aerosols on surface UV radiation is clarified. For this reason, the second part of this work focuses on the relation between the erythemal UV dose, global solar radiation, total ozone column and AOD (at 320 nm) at Uccle. Simultaneous measurements of these variables are available for a time period of 25 years (1991–2015) and this time series is long enough to allow for reliable determination of significant changes. Different analysis techniques (linear trend analysis, change point analysis and multiple linear regression) are combined to allow for an extensive study of the relations between the variables., Doctorat en Sciences, info:eu-repo/semantics/nonPublished

Solar ultraviolet (UV) radiation has a broad range of effects concerning life on Earth. Soon after the mid-1980s, it was recognized that the stratospheric ozone content was declining over large areas of the globe. Because the stratospheric ozone layer protects life on Earth from harmful UV radiation, this lead to concern about possible changes in the UV radiation due to anthropogenic activity. Initiated by this concern, many stations for monitoring of the surface UV radiation were founded in the late 1980s and early 1990s. As a consequence, there is an apparent lack of information on UV radiation further in the past: measurements cannot tell us how the UV radiation levels have changed on time scales of, for instance, several decades. The aim of this thesis was to improve our understanding of past variations in the surface UV radiation by developing techniques for UV reconstruction. Such techniques utilize commonly available meteorological data together with measurements of the total ozone column for reconstructing, or estimating, the amount of UV radiation reaching Earth's surface in the past. Two different techniques for UV reconstruction were developed. Both are based on first calculating the clear-sky UV radiation using a radiative transfer model. The clear-sky value is then corrected for the effect of clouds based on either (i) sunshine duration or (ii) pyranometer measurements. Both techniques account also for the variations in the surface albedo caused by snow, whereas aerosols are included as a typical climatological aerosol load. Using these methods, long time series of reconstructed UV radiation were produced for five European locations, namely Sodankylä and Jokioinen in Finland, Bergen in Norway, Norrköping in Sweden, and Davos in Switzerland. Both UV reconstruction techniques developed in this thesis account for the greater part of the factors affecting the amount of UV radiation reaching the Earth's surface. Thus, they are considered reliable and trustworthy, as suggested also by the good performance of the methods. The pyranometer-based method shows better performance than the sunshine-based method, especially for daily values. For monthly values, the difference between the performances of the methods is smaller, indicating that the sunshine-based method is roughly as good as the pyranometer-based for assessing long-term changes in the surface UV radiation. The time series of reconstructed UV radiation produced in this thesis provide new insight into the past UV radiation climate and how the UV radiation has varied throughout the years. Especially the sunshine-based UV time series, extending back to 1926 and 1950 at Davos and Sodankylä, respectively, also put the recent changes driven by the ozone decline observed over the last few decades into perspective. At Davos, the reconstructed UV over the period 1926-2003 shows considerable variation throughout the entire period, with high values in the mid-1940s, early 1960s, and in the 1990s. Moreover, the variations prior to 1980 were found to be caused primarily by variations in the cloudiness, while the increase of 4.5 %/decade over the period 1979-1999 was supported by both the decline in the total ozone column and changes in the cloudiness. Of the other stations included in this work, both Sodankylä and Norrköping show a clear increase in the UV radiation since the early 1980s (3-4 %/decade), driven primarily by changes in the cloudiness, and to a lesser extent by the diminution of the total ozone. At Jokioinen, a weak increase was found, while at Bergen there was no considerable overall change in the UV radiation level. Auringon ultraviolettisäteily (UV-säteily) vaikuttaa usealla tavalla elämään maan päällä. 1980-luvun puolivälin jälkeen huomattiin, että stratosfäärin otsonimäärä oli vähenemässä etenkin Etelämantereen kevätkaudella mutta myös maapallonlaajuisesti. Stratosfäärin otsonikerros suojelee elämää maan päällä haitalliselta UV-säteilyltä, ja havaitut otsonikerroksen muutokset aiheuttivat huolta ihmiskunnan mahdollisesti aiheuttamista muutoksista UV-säteilymäärissä. Tämän seurauksena useimmat UV-säteilyn mittausasemat ovat perustettuja juuri tähän aikaan 1990-luvun taitteessa. UV-säteilyn mittausaikasarjat ovat siis melko lyhyitä, ja ne pystyvät tyypillisesti kertomaan meille UV-säteilyn vaihteluista vain viimeisten noin 15 vuoden ajalta. Tämän väitöskirjatyön tavoitteena oli tuottaa uutta tietoa UV-säteilyn vaihteluista menneisyydessä kehittämällä ns. UV-rekonstruointimenetelmiä, joissa hyödynnetään yleisiä meteorologisia mittauksia ja kokonaisotsonitietoa menneen ajan UV-säteilyn arvioimiseen. Tässä työssä kehitettiin kaksi UV-rekonstruointimenetelmää. Molemmissa lasketaan aluksi säteilynkuljetusmallilla pilvettömän sään UV-säteilymäärä. Pilvien vaikutus otetaan tämän jälkeen huomioon joko auringon paistehavaintojen tai pyranometrimittauksien perusteella. Lisäksi kumpikin menetelmä ottaa huomioon lumen aiheuttamat vaihtelut maan pinnan heijastuvuudessa. Ilmakehän pienhiukkaset ovat mukana laskuissa tyypillisenä määränä kullakin paikkakunnalla. Näitä kahta menetelmää käyttäen tuotettiin pitkiä aikasarjoja menneen ajan UV-säteilystä viidelle asemalle Euroopassa. Asemat olivat Sodankylä ja Jokioinen Suomessa, Bergen Norjassa, Norrköping Ruotsissa ja Davos Sveitsissä. Kumpikin tässä työssä kehitetty menetelmä ottaa huomioon tärkeimmät UV-säteilymäärään vaikuttavat tekijät ja tulokset ovat hyviä verrattaessa riippumattomiin havaintoihin. Tämän vuoksi menetelmiä voidaan pitää luotettavina. Pyranometrimittauksiin perustuva menetelmä on tarkempi kuin paistehavaintoihin perustuva etenkin päiväkohtaisia arvoja verrattaessa. Kuitenkin paistehavaintoihin perustuva menetelmä on kuukausiarvoja tarkasteltaessa lähes yhtä tarkka kuin pyranometrimenetelmä, mikä tarkoittaa että paistemenetelmä on suurin piirtein yhtä hyvä kuin pyranometrimenetelmä arvioitaessa pidemmän aikavälin vaihteluita kuten esimerkiksi vuosi vuodelta tapahtuvaa vaihtelua. Tässä työssä tuotetut pitkät UV-aikasarjat tuovat uutta tietoa UV-säteilyn ilmastollisesta käyttäytymisestä ja siitä kuinka UV-säteily on vaihdellut menneisyydessä. Esimerkiksi auringon paistehavaintoihin perustuvat aikasarjat ulottuvat vuoteen 1926 Davosissa ja vuoteen 1950 Sodankylässä. Näin ollen ne muodostavat myös uuden vertailukohdan viimeaikaisille muutoksille, joissa otsonikadolla on ollut merkitystä (noin 1980 alkaen). Davosissa UV-säteily on vaihdellut tuntuvasti koko tarkastelujaksolla 1926-2003. Korkeita arvoja oli 1940-luvun keskivaiheilla, 1960-luvun alussa ja 1990-luvulla. Lisäksi huomattiin, että pilvisyyden vaihtelut hallitsivat ennen vuotta 1980 tapahtuneita vaihteluita UV-säteilyssä. Toisaalta sekä pilvisyys että otsonin vähentyminen vaikuttivat jakson 1979-1999 aikana todettuun kasvuun UV-säteilyssä (4,5 %/vuosikymmen). Myös Sodankylässä ja Norrköpingissä UV-säteily on lisääntynyt 1980-luvun alusta (3-4 %/vuosikymmen). Näillä asemilla kasvun aiheutti ensisijaisesti pilvisyyden muutokset ja vähemmässä määrin otsonin vähentyminen. Jokioisissa ja Bergenissä UV-säteilyn muutokset olivat pieniä.